Controllable
Synthesis of Supported PdAu Nanoclusters
and Their Electronic Structure-Dependent Catalytic Activity in Selective
Dehydrogenation of Formic Acid
posted on 2021-07-15, 09:29authored byWanyue Ye, He Huang, Wenhui Zou, Yuzhen Ge, Rongwen Lu, Shufen Zhang
We
report the design and synthesis of uniform PdAu alloy nanoclusters
immobilized on diamine and graphene oxide-functionalized silica nanospheres.
The structure-dependent activity for selectively catalytic dehydrogenation
of formic acid (FA) has been evaluated and optimized by controlling
the Pd/Au mole ratio and the carrier components. The relationship
between the catalyst structure and activity has been investigated
via both experiments and characterization. High-resolution transmission
electron microscopy (TEM) and X-ray diffraction (XRD) proved the formation
of PdAu alloy nanoclusters. In situ diffuse reflectance infrared Fourier
transform spectroscopy (DRIFTS), X-ray photoelectron spectroscopy
(XPS), and X-ray absorption fine structure (XAFS) analyses verified
the electron transfer between Au, Pd, and the support. An outstanding
turnover frequency (TOF) value of 16 647 h–1 at 323 K, which is among the highest activity for FA dehydrogenation
ever reported, can be achieved at optimized conditions and ascribed
to the combination of the bimetallic synergistic effect and the carrier
effect.